This study aimed to investigate the effects of acid or alkali modification of isolated cassava starch (ICS) on its physicochemical properties. Acetic acid concentrations of 5%, 10%, and 20% v/v (0.87, 1.73, and 3.46 M, respectively) and calcium hydroxide concentrations of 0.15%, 0.20%, and 0.30% w/w (0.02, 0.025, and 0.04 M, respectively) were tested independently and compared with untreated isolated starch. The scanning electron microscope (SEM) shows starches with polyhedral and semispherical shapes; these modifications do not change the surface of the starch granules. Nanocrystals with orthorhombic crystal structure were extracted from ICS. Transmission electron microscopy (TEM) shows crystallites with a size (two‐dimensional) of 20 ± 5 nm in length and 10 ± 2 nm in width and reveals that this starch contains nanocrystals with orthorhombic crystal structure. The X‐ray patterns show that these nanocrystals are unaffected by acidic or alkaline treatments. The Ca+2 and CH3COO− ions do not interact with these nanocrystals. The alkaline treatment only affects the gelatinization temperature at a Ca(OH)2 concentration of 0.30%. Low concentrations of acidic and alkaline treatments affect the ability of cassava starch to absorb water and reduce the peak and final viscosity. The infrared spectra show that the modifications lead to C–H and C═C bond formations. ICS‐B 0.30 can modify the amorphous regions of the starch, and the acid treatment leads to acetylation, which was confirmed by the presence of an IR band at 1740 cm−1.